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Gas-phase vs. material-kinetic limits on the redox response of nonstoichiometric oxides

Ji, Ho-Il and Davenport, Timothy C. and Ignatowich, Michael J. and Haile, Sossina M. (2017) Gas-phase vs. material-kinetic limits on the redox response of nonstoichiometric oxides. Physical Chemistry Chemical Physics, 19 (10). pp. 7420-7430. ISSN 1463-9076. doi:10.1039/c7cp00449d.

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Cerium dioxide, CeO_(2−δ), remains one of the most attractive materials under consideration for solar-driven thermochemical production of chemical fuels. Understanding the rate-limiting factors in fuel production is essential for maximizing the efficacy of the thermochemical process. The rate of response is measured here via electrical conductance relaxation methods using porous ceria structures with architectural features typical of those employed in solar reactors. A transition from behavior controlled by material surface reaction kinetics to that controlled by sweep-gas supply rates is observed on increasing temperature, increasing volume specific surface area, and decreasing normalized gas flow rate. The transition behavior is relevant not only for optimal reactor operation and architectural design of the material, but also for accurate measurement of material properties.

Item Type:Article
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Ji, Ho-Il0000-0002-6194-991X
Haile, Sossina M.0000-0002-5293-6252
Additional Information:© 2017 the Owner Societies. Received 20th January 2017; Accepted 22nd February 2017; First published online 22 Feb 2017. This material is based upon work supported by the U.S. Department of Energy, through ARPA-e Contract DE-AR0000182. This work was also partially supported by the IMI Program of the National Science Foundation under Award No. DMR 08-43934. We gratefully acknowledge Dr Jie Yin and Prof. Xue-Jian Liu of the Shanghai Institute of Ceramics, Chinese Academy of Sciences, for instruction in RPC fabrication. Microstructure analysis made use of the EPIC facility of Northwestern University’s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205).We thank Dr Xianghui Xiao for performing X-ray tomography, using resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Porosimetry results were kindly provided by staff at Micromeritics Analytical Services, Norcross, GA.
Funding AgencyGrant Number
Department of Energy (DOE)DE-AR0000182
NSFDMR 08-43934
Department of Energy (DOE)DE-AC02-06CH11357
Issue or Number:10
Record Number:CaltechAUTHORS:20170228-103323936
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:74591
Deposited By: Tony Diaz
Deposited On:28 Feb 2017 19:23
Last Modified:11 Nov 2021 05:28

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